Oxygen and hydrogen peroxide reduction catalyses in neutral aqueous media using copper ion loaded glassy carbon electrode electrolyzed in ammonium carbamate solution

Oxygen and hydrogen peroxide reduction catalyses in neutral aqueous media using copper ion loaded glassy carbon electrode electrolyzed in ammonium carbamate solution
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DOI:
10.1016/j.electacta.2008.09.020
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发表时间:
2009-01-30
影响因子:
6.6
通讯作者:
Uchiyama, Shunichi
Uchiyama, Shunichi
中科院分区:
材料科学2区
文献类型:
--
作者:
Watanabe, Hiroaki;Yamazaki, Haruhito;Uchiyama, Shunichi

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通过在氨基甲酸铵溶液中对玻碳电极进行电极氧化,可以得到氨基化玻碳电极。在循环伏安实验中,当使用氨基化玻碳电极作为工作电极时,溶解氧的电极还原从中性水介质中-0.15V vs. Ag/AgCl开始,而当使用抛光GCE时,溶解氧的电极还原从-0.40V vs. Ag/AgCl开始。氨基甲酸电极氧化引入的含氮基团必然与氧的电子转移速率加快有关。此外,当铜(11)离子配位到AGCE表面时,在+0.15V vs. Ag/AgCl下出现了新的溶解氧还原波。氧的还原电位与铜(11)离子的还原电位一致,这表明铜离子在胺化碳表面的配位是氧的氧化还原介质。通过旋转铂环胺化玻碳圆盘电极对氧的还原产物进行监测,发现在-0.4 v vs. Ag/AgCl的负电位范围内,大部分氧被还原为水。通过AGCE,发现过氧化氢的催化还原和氧还原也发生了。(C) 2008 Elsevier Ltd版权所有。
An aminated glassy carbon electrode (AGCE) can be obtained by the electrode oxidation of glassy carbon electrode in ammonium carbamate solution. In the cyclic voltammetric experiments, the electrode reduction of the dissolved oxygen began from -0.15V vs. Ag/AgCl in neutral aqueous media when the aminated glassy carbon electrode was used as a working electrode although it began from -0.40V vs. Ag/AgCl when a polished GCE was used. The nitrogen containing groups introduced by the electrode oxidation of carbamic acid must be related with the acceleration of the electron transfer rate of oxygen. Moreover, the new reduction wave of the dissolved oxygen appeared at +0.15V vs. Ag/AgCl when copper (11) ion was coordinated to AGCE surface. This reduction potential of oxygen coincided with that of copper (11) ion and this fact suggests that the coordinated copper ion to the aminated carbon surface works as a redox mediator of oxygen. The reduction product of oxygen was monitored by rotating platinum ring - aminated glassy carbon disk electrode, and it was found that most of oxygen was reduced to water in a potential range negative than -0.4V vs. Ag/AgCl. By using AGCE, it was recognized that the catalytic reduction of hydrogen peroxide was also taken place as well as oxygen reduction. (C) 2008 Elsevier Ltd. All rights reserved.